Abstract

AbstractCalcium sulfate (CaSO4), an essential retarder in cement, retards the hydration of tricalcium aluminate (C3A) and tetracalcium aluminoferrite (C4AF) phases. However, its retarding mechanism remains unclear. This paper focused on the adsorption of CaSO4f on C4AF and C3A surfaces based on isothermal calorimetry, the measurement of the ionic concentrations in a diluted system, and density functional theory to enhance the understanding of the retardation mechanism. The results showed that the retarding effect of CaSO4 on C4AF was stronger than that on C3A due to the slower CaSO4 consumption rate, lower driving force for CaSO4 adsorption, and surface coverage of Fe(OH)3 gel. The adsorption of CaSO4 hindered Ca dissolution more markedly on C4AF than C3A, which was pronounced on Fe‐free C4AF surfaces. The adsorption of CaSO4 weakened the affinity of water on C4AF and C3A surfaces, lowering the driving force for H2O adsorption. The adsorption of H2O and CaSO4 promoted the dissolution of Al on the [AlO6] octahedral surface of C4AF, which may be responsible for the maintenance of a higher Al concentration in the solution. Based on the above results, the adsorption of CaSO4 on initial C4AF and C3A hydration was explained.

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